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Early-stage latent thermal failure of single-crystal Ni-rich layered cathode

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High nickel content worsens the thermal stability of layered cathodes for lithium-ion batteries,raising safety concerns for their applications.Thoroughly understanding the thermal failure process can offer valuable guidance for material optimization on thermal stability and new opportunities in monitoring battery thermal runaway(TR).Herein,this work comprehensively investigates the thermal failure pro-cess of a single-crystal nickel-rich layered cathode and finds that the latent thermal failure starts at～120 ℃ far below the TR temperature(225 ℃).During this stage of heat accumulation,sequential structure transition is revealed by atomic resolution electron microscopy,which follows the layered → cation mixing layered → LiMn2O4-type spinel → disordered spinel → rock salt.This progres-sion occurs as a result of the continuous migration and densification of transition metal cations.Phase transition generates gaseous oxygen,initially confined within the isolated closed pores,thereby not showing any thermal failure phenomena at the macro-level.Increasing temperature leads to pore growth and coalescence,and eventually to the formation of open pores,causing oxygen gas release and weight loss,which are the typical TR features.We highlight that latent thermal instability occurs before the macro-level TR,suggesting that suppressing phase transitions caused by early thermal instability is a cru-cial direction for material optimization.Our findings can also be used for early warning of battery thermal runaway.

Thermal runawayNickel-rich layered cathodeTransmission electron microscopyLithium-ion batteryPhase transition

Xiao Han、Ruoyu Xu、Yan Li、Yang Ding、Manchen Zhang、Bo Wang、Xiaoxing Ke、Manling Sui、Pengfei Yan

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Beijing Key Laboratory of Microstructure and Property of Solids,Faculty of Materials and Manufacturing,Beijing University of Technology,Beijing 100124,China

Watt Laboratory,Central Research Institute,Huawei Technologies Co.,LTD,Shenzhen 518129,Guangdong,China

National Natural Science Foundation of ChinaNatural Science Foundation of Beijing,ChinaChina National Petroleum Corporation Innovation FoundNational Natural Science Foundation of ChinaNational Natural Science Foundation of China

1217401522120032021DQ02-10041207401712274010

2024

10.1016/j.jechem.2024.05.020

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.96(9)